Material Discovery and Design Principles for Stable, High Activity Perovskite Cathodes for Solid Oxide Fuel Cells

Abstract Critical to the development of improved solid oxide fuel cell (SOFC) technology are novel compounds with high oxygen reduction reaction (ORR) catalytic activity and robust stability under cathode operating conditions. Approximately 2145 distinct perovskite compositions are screened for potential use as high activity, stable SOFC cathodes, and it is verified that the screening methodology qualitatively reproduces the experimental activity, stability, and conduction properties of well‐studied cathode materials. The calculated oxygen p ‐ band center is used as a first principle‐based descriptor of the surface exchange coefficient ( k* ), which in turn correlates with cathode ORR activity. Convex hull analysis is used under operating conditions in the presence of oxygen, hydrogen, and water vapor to determine thermodynamic stability. This search has yielded 52 potential cathode materials with good predicted stability in typical SOFC operating conditions and predicted k* on par with leading ORR perovskite catalysts. The established trends in predicted k* and stability are used to suggest methods of improving the performance of known promising compounds. The material design strategies and new materials discovered in the computational search help enable the development of high activity, stable compounds for use in future solid oxide fuel cells and related applications.